Dissolvable Films Impregnated with Encapsulated Tobacco, Tea, Coffee, Botanicals, and Flavors for Oral Products

ABSTRACT

A process for preparing an orally-enjoyable film of encapsulated plant material includes combining particles of finely divided plant material, a first coating material, and a second coating material, then inducing gelation to form a gel matrix of the particles coated with the first coating material embedded in the second coating material, followed by forming a film from the gel matrix. Also disclosed is a film of coated particles of finely-divided plant material, made of a gel matrix of plant material at least partially surrounded by a first coating material and embedded in a second coating material.

CROSS REFERENCE TO RELATED APPLICATIONS

This application claims priority under 35 U.S.C. §119 to U.S.Provisional Application No. 61/141,557 entitled DISSOLVABLE FILMSIMPREGNATED WITH ENCAPSULATED TOBACCO, TEA, COFFEE, BOTANICALS, ANDFLAVORS FOR ORAL PRODUCTS, filed Dec. 30, 2008, the entire content ofwhich is hereby incorporated by reference.

SUMMARY

In one embodiment, a process is provided for preparing a film of coatedparticles of finely-divided plant material, comprising: combiningparticles of finely divided plant material and a first coating materialin a liquid medium, wherein the first coating material adsorbs onto atleast a portion of a surface of the particles to form a layer of thefirst coating material; mixing a second coating material with the liquidmedium, wherein the second coating material adsorbs onto at least aportion of the layer; inducing gelation to form a gel matrix comprisingthe particles at least partially surrounded by the layer of the firstcoating material and embedded in the second coating material; andforming a film from the gel matrix, wherein (i) the plant material andthe first coating material are electrostatically attracted, (ii) thefirst coating material and the second coating material areelectrostatically attracted, or (iii) both (i) and (ii).

In another embodiment, a film of coated particles of finely-dividedplant material is provided, the film comprising: a gel matrix comprisingparticles of finely-divided plant material at least partially surroundedby a first coating material and embedded in a second coating material,wherein (i) the plant material and the first coating material areelectrostatically attracted, (ii) the first coating material and thesecond coating material are electrostatically attracted, or (iii) both(i) and (ii).

In a particular embodiment, the finely divided particles of plantmaterial are coated with plant-sourced proteins and/or plant-sourcedpolysaccharides, for example tobacco sourced pectins.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 is a schematic illustration of a film of coated particles asdescribed herein.

FIG. 2 is a schematic diagram of a method for preparing a film of coatedparticles as described herein.

DETAILED DESCRIPTION

The present application describes processes for preparingorally-enjoyable films of coated particles of plant material. In aparticular embodiment, ground tobacco particles are coated withpolysaccharide-protein coacervate gels and formed into films.

For increased consumer acceptability of orally utilized compositions ofplant materials, the materials are coated to improve their mouth feel,taste, texture, appearance, smell, flavor and/or flavor delivery, orother attributes.

Plant materials that may be encapsulated include smokeless tobaccos,comprising chewing tobacco, snus, dry snuff, and moist snuff, as well asnon-tobacco botanicals such as coffee or tea. Encapsulation to formfilms as described herein can offset negative flavor characteristics(such as bitterness, astringency, acridness, flavor harshness, and/orunpleasant aftertaste) of orally enjoyable products that include plantmaterials.

Films as described herein provide numerous advantages. Because coatingmaterials comprising the film supply a neutral aesthetic color over thebase particle of plant material (as opposed to the deep brown color of,e.g., ground tobacco particles), the films can be incorporated intoproducts without the need for added colorants. Optionally, color may beadded to the neutral base color of one or more coatings in the film. Thecoated particles making up the film also exhibit reduced odor comparedto, e.g., uncoated tobacco particles. Additionally, a coating asdescribed herein may provide for improved cohesion, thus aiding in theformation of a film.

Moreover, when the coated particles are in the mouth, they swell uponmixture with saliva, creating a pleasant mouthfeel, and reducing certainundesired physiological sensations, such as throat itching, that cansometimes be observed when uncoated tobacco products are used. Theparticles provide a mild, creamy flavor and texture that combinesparticularly well with other food ingredients, such as sugars, starches,polyols, oils, lipids, waxes, fats, fatty acids, glycerides, etc.

A film of coated particles as described herein advantageously providescontrolled release of flavors from the plant material, while alsopermitting control of the time profile of flavorant release byadjustment of the integrity and thickness of the coatings, and of thegel strength. In a particular embodiment, wherein coating materials areat least partially derived from tobacco, economic efficiencies areobtained as well, since they can replace other materials that mightotherwise result in greater costs.

As used herein, the term “film” denotes a relatively flat article,including a strip, a tape, a sheet, and the like.

As used herein, the term “coacervate” denotes aggregations of moleculesheld together via non-covalent interactions such as electrostatic, vander Weals and hydrophobic attractive forces, and the like. A specificexample of a coacervate is one or more particles of plant material, suchas tobacco particles, that are held to an aggregation of proteinmolecules (typically electrostatically charged) that form a coating onat least part of the surface of the particles and form a layer. Theseprotein molecules in turn bind to an aggregation of polysaccharidemolecules that substantially surround the layer.

As used herein, the term “particle” denotes a relatively small,subdivided unit of material, which may be in one or more of a variety ofregular or irregular shapes. The term is intended to include powders,granules, shreds, and elongated structures, such as whiskers, fibers,and the like. The term is also intended to include droplets of liquid orgel, e.g., droplets of liquid plant extract, as well as solids.

As used herein, the terms “colloidal” and “colloid” refer to a system inwhich finely divided particles, which are approximately 10 to 10,000angstroms in size, are dispersed within a continuous medium in a mannerthat prevents them from being filtered easily or settled rapidly.

As used herein, the term “finely divided” denotes particles whichpossess an average size of about 3000 μm or less. To “finely divide” amaterial denotes processing by comminution, pulverization, grinding,micronization, cutting, shredding, and the like, to produce a finelydivided material.

As used herein, the term “orally enjoyable” denotes the ability of amaterial or product to be enjoyed and at least partially consumed viathe mouth.

As used herein, the term “about” when used in conjunction with a statednumerical value or range denotes somewhat more or somewhat less than thestated value or range, to within a range of ±10% of that stated.

Plant Material Particles

Any plant or botanical material typically consumed by humans or animalscan be coated by the methods described herein. Particularly suitableplant materials include tobacco and tobacco substitutes. The plantmaterials are generally in particulate form, and are preferably under 3mm in size, more preferably under 1000 microns in size. The term“micronized” as used herein means reduced to an average size of nolarger than about 250 microns.

Suitable particles of plant material may include, or be derived from,any part of a plant, such as leaf, stem, flower, fruit, nut, bean, bark,root, and the like. The term “derived from,” as used herein, is intendedto include any materials obtained by processing plant part(s) itself,such as extract fractions of a plant (e.g., an extract of a tobaccoplant) or parts thereof. The plant material may be ground, shredded, orotherwise processed to obtain particles from larger pieces of plantmaterial. The particles may be in any suitable form including, but notlimited to, shreds, granules and powders, and can have any desiredshape, such as different regular and irregular shapes. Suitable regularshapes may include round, square, rectangular, oval, other polygonalshapes, cylindrical, fibrous, and the like.

In one embodiment, the particles of plant material take the form offinely-divided powders, such as tobacco powders. Preferably, theparticles can have a diameter less than about 3 mm, and more preferablyless than about 1000 microns, and even more preferably, between about0.2 microns and about 250 microns, and most preferably, between about 1micron and about 100 microns. In a further embodiment, the particles caninclude ground or micronized particles of a size so that they can form acolloidal suspension of particles in a liquid medium, more particularlyin an aqueous medium, such as water. In forming the coating as describedbelow, the particles can be added in the form of a powder or as acolloidal dispersion.

In a particular embodiment, the particles of plant material can beelectrostatically charged, Zwitterionic, or neutral. Electrostaticallycharged particles can more easily attract and hold one or more proteinsto form a coacervate. If the finely divided plant material does not havethe desired innate charge for attracting the protein coating material,the particles may be treated to alter the charge thereof before beingmixed with the protein coating material, as described in more detailherein. In a particular embodiment, the particles desirably have anegative overall electrostatic charge. Ground tobacco particlesgenerally have a net negative electrostatic charge if untreated.

First Coating

The first coating material may be selected from the group consisting ofproteins (which includes protein hydrolyzates), cationic polysaccharidesor oligosaccharides, non-ionic polysaccharides, or oligosaccharides, andmixtures of them. It is desirable to select a first coating materialthat has a charge that will be attracted to the charge possessed by thedivided plant material.

In one aspect there is provided a coated particle of plant materialwhich comprises a base particle of finely-divided plant material whichcan be charged or neutral, a first coating material coating at least aportion of, and preferably all of, the base particle and a secondcoating material disposed at least partially on said first coatingmaterial. The first coating material can be neutral, Zwitterionic, orionic, preferably cationic. The first coating material is preferablyselected from the group consisting of proteins (including proteinhydrolyzates), cationic polysaccharides, cationic oligosaccharides,non-ionic polysaccharides, non-ionic oligosaccharides, and mixtures ofthem. The second coating material can also be ionic, Zwitterionic, orneutral.

The first coating material may comprise (i) a protein or proteinhydrolyzate, especially a zwitterionic or cationic protein in the casewhere the plant material is negatively charged; (ii) a cationicpolysaccharide (especially when the plant material is negativelycharged), preferably a cationic polysaccharide selected from the groupconsisting of chitosan, quaternary cellulosic polymers, modifiedcationic polysaccharides, polyquat-4, amidated pectins, and amidated orcationically modified starches; or (iii) non-ionic polysaccharide, apolyvinyl pyrrolidone, a poly vinyl alcohol, or combinations thereof. Ifthe first coating material is a non-ionic polysaccharide, it may beselected from the group consisting of modified starches, or methylcellulose and derivatives thereof, including hydroxyl propyl methylcellulose, propylene glycol ester of alginic acid, agar, curdlan, andmodified pectins, such as those of citrus, apple, plum, gooseberry, ortobacco plant origin. Combinations of two or more of these materials maybe used.

If the first coating material is a protein, it may be a plant-based oranimal-based protein, and preferably is, or is derived from, a milkprotein, a fish gelatin, a whey protein, an egg white protein, a riceprotein, a soy protein, a wheat protein, a tobacco protein or a proteinfraction from a tobacco plant, a protein from or derived from tobaccoextract, or combinations thereof, a gelatin other than fish gelatin,corn protein, or protein hydrolyzates. The protein may contain a highcontent of amino acid groups with a nitrogen-containing (preferablynon-cyclic) side chain, such as lysine, asparagine, glutamine, andarginine, which are beneficial for crosslinking with carbohydratecarboxylic groups under processing conditions. Gelatins other than fishgelatin include beef gelatin, pork gelatin, and gelatin hydrolyzates.Fish gelatin, for example, can be produced by comminution of the mincedflesh of any of several species of lean fish, e.g., haddock, cod, cusk,cat and ocean perch. During comminution a small amount of sodiumchloride may be added to improve the texture of the finished fishgelatin product.

In a particular embodiment, the protein desirably has a molecular weightranging between about 2 kDa and about 1000 kDa, and preferably betweenabout 15 kDa and about 500 kDa.

The protein coating material can have an overall electrostatic charge,or can be zwitterionic or neutral. It is desirable to select a proteincoating material that has an electrostatic charge opposite a chargepossessed by the particles of plant material. Charges on the protein canfacilitate electrostatic complexation between the protein-coatedparticle and a subsequent polysaccharide coating, thereby helping toform the coacervate. In one embodiment, the protein coating material canbe zwitterionic or cationic in the case where the tobacco material hasan overall negative electrostatic charge. The electrostatic charge onthe protein can be modified by placing the protein in an aqueoussolution, and adjusting the pH of the solution until the desired chargeis obtained. The pH adjustment necessary and the resulting electrostaticcharge obtained depend, to some extent, on the pKa of the protein sidechains. For example, acidifying the protein solution (so that pH<pKa ofthe acidic and basic side chains) will generally place a net positiveelectrostatic charge on the protein, while making the protein solutionmore alkaline (pH>pKa of the acidic and basic side chains) willgenerally result in proteins having a net negative electrostatic charge.

If an allergen-free product is desired, it is preferred to employprotein derived from fish gelatin, rice protein, oat protein, or cornprotein, or their hydrolyzates. It is preferable that the proteins berelatively pure and not treated or “instantized” with surfactants. Itmay also be preferable to treat the protein or protein hydrolyzatecoating with an acid to impart a positive charge to facilitateelectrostatic complexation between the protein and a subsequent coatingcomprising a polysaccharide/oligosaccharide.

The first coating material may have a molecular weight between about 2kDa and about 1000 kDa, or preferably between about 15 kDa and about 500kDa.

Second Coating

The second coating material is adsorbed over at least a portion of, andpreferably all of, the first coating. As a result, a gel matrix can beobtained comprising the plant particles at least partially surrounded bythe layer of the first coating material, and embedded in the secondcoating material. Here, “embedded in” means that the second coatingmaterial substantially surrounds the layer of first coating materialwhich is around the plant particle. The second coating may be thought ofas a continuous phase of the gel matrix.

The second coating material may be ionic, zwitterionic or neutral. Moreparticularly, the second coating material preferably comprises ananionic, zwitterionic or neutral polysaccharide, a protein (includingprotein hydrolyzates), a mixture of polysaccharides, or a mixture of oneor more polysaccharides and one or more proteins. The second coatingmaterial may have a molecular weight between about 5 kDa and about 1,000kDa, preferably between about 100 kDa and about 500 kDa, more preferablybetween about 200 kDa and about 500 kDa.

If the second coating material is an anionic or zwitterionicpolysaccharide, it is preferably selected from at least one ofcarrageenan, gum Arabic, carboxymethyl cellulose, pectins, such as thosefrom citrus, apple, plum, gooseberry or tobacco plant origin, sodiumalginate, gum tragacanth, locust bean gum, gellan gum, and xanthan gum.

If the second coating is a nonionic polysaccharide, it is preferablyselected from the group consisting of modified starches, methylcellulose and derivatives thereof, hydroxy propyl methyl cellulose,propylene glycol ester of alginic acid, agar, curdlan, and modifiedpectins of citrus, apple, plum, gooseberry, or tobacco plant origin(where the pectins have been modified to be non-ionic).

If the second coating is a protein, it may be either plant or animalbased, and is preferably derived from milk protein, whey protein, eggwhite protein, soy protein, rice protein, wheat protein, tobacco proteinfractions from tobacco plants or tobacco extracts, fish gelatin, gelatinother than fish gelatin, corn protein, or protein hydrolyzates. If it isdesired to provide allergen-free products, the protein may be derivedfrom rice, fish gelatin, oat protein, corn protein, or theirhydrolyzates. The protein preferably has a net negative or neutralcharge under solution pH.

A polysaccharide having a net negative electrostatic charge is desirablebecause it forms a stable coacervate with a positively charged proteinlayer. If desired, the charge on the polysaccharide can be manipulatedby, e.g., adjusting the pH of a liquid medium containing thepolysaccharide.

The polysaccharide to be used as a coating is preferablynon-standardized (i.e., supplied in a form without additives) andsubstantially free of salts, sugars, and hemicelluloses (e.g., compoundswith a molecular weight of between about 1 kDa to about 5 kDa). In aparticular embodiment, suitable polysaccharides preferably have amolecular weight ranging between about 5 kDa and about 1,000 kDa, morepreferably between about 100 kDa and about 500 kDa, and most preferably,between about 200 kDa and about 500 kDa.

Preferably, at least one of the polysaccharides or proteins in thesecond coating can form a gel in the pH range of about 3 to about 9.Alternatively, or in addition, it is preferred that the second coatingmaterial further comprises one or more monovalent, divalent, ortrivalent cations such as potassium, calcium, magnesium, and iron, inthe form of salts such as chloride, citrate, lactate or acetate salts,which may assist in forming salt bridges between the coating materials,particularly when the second coating material includes an anionic orneutral polysaccharide, a protein, a mixture of polysaccharides, or amixture of polysaccharide and protein. Alternatively, or in addition,the proteins and polysaccharides of the second coating can gel as aresult of crosslinking, hydrogen bonding, hydrophobic interactions, orelectrostatic complexation, particularly among carboxylic groups ofpolysaccharides and amino groups of proteins, or vice versa.

If desired, the protein or protein hydrolyzate of the second coatingmaterial can be converted to a positive charge to facilitateelectrostatic complexation between the protein and thepolysaccharide/oligosaccharide. The conversion of the protein to arelatively positive state may be affected by lowering the pH of theliquid medium with weak food grade organic acids such as acetic, adipic,fumaric, malic, lactic, tartaric, and/or gluconic acids, gluco deltalactone, and/or food grade inorganic acids such as strong hydrochloricacid.

Control of the kinetics of extraction can be exercised by manipulatingthe gel strength of the second coating. Gel strength can be controlledby, e.g., controlling the molecular weight, polydispersity, degree ofesterification, degree of pectin amidation (in particular, the degree ofamidation of tobacco-derived pectins), combining pectins withcarageenans, and/or by manipulating the processing of the coatedparticles, and in particular, the order of addition of polysaccharidesand/or proteins.

Coating the Particle and Gelation

One embodiment includes a method for preparing coated particles offinely-divided plant material, comprising combining in a liquid mediumparticles of plant material and a first coating material, wherein thefirst coating material adsorbs onto at least a portion of a surface ofthe particles to form a layer, and mixing a second coating material withthe liquid medium, wherein the second coating material adsorbs onto atleast a portion of the layer. Subsequently, as described below, themixture is gelled and a film of encapsulated plant material formed.

In a particular embodiment of this method, the combining comprisesadding either the particles of plant material, or a colloidal dispersionof the particles of divided plant material in a dispersing medium, to adispersion of the first coating material in the first liquid medium. Thedispersing medium is preferably an aqueous medium, such as deionizedwater.

The formation of the coatings typically involves the gelling of thefirst and/or second coating material. This may be accomplished by, e.g.,adjusting the pH of the coating material or the surrounding liquidmedium or both, adjusting the temperature of the coating material or thesurrounding liquid medium or both, introducing gelation agents, or acombination of these. Different methods may be used to gel each coatingmaterial.

The particles of plant material are typically naturallynegatively-charged, and thus disposed to electrostatically attract apositively-charged first coating material (e.g., a protein). However, ifthe particles are not negatively-charged as obtained, they may betreated with appropriate reagents to impart a negative charge to theparticles before they are mixed with the first coating. For example,particles may be treated with an appropriate amount of one or more basessuch as sodium carbonate, sodium bicarbonate, and/or sodium hydroxide(such as lye), to impart a negative charge to at least some of theparticle surfaces.

The suitably micronized plant material can be dispersed in a dispersingmedium, preferably an aqueous medium (e.g., deionized water), to form acolloidal dispersion of the plant material. The plant material dispersedin the dispersing medium can be added to a solution of the first coatingmaterial in the liquid medium to form a coated particle dispersed in theliquid medium. Alternatively, the micronized plant material can be addeddirectly to the first coating material in the liquid medium to form thecoated plant material dispersed in the liquid medium.

The pH of either the dispersed plant material or the first coatingmaterial can be altered relative to the liquid medium, e.g., byadjusting the pH of the liquid medium as desired to facilitate theelectrostatic coating of the plant material. Suitable substances foradjusting the pH include food-grade materials such as weak organicacids, e.g., acetic acid, adipic acid, fumaric acid, malic acid, lacticacid, tartaric acid, or gluconic acid, or mixtures of these, or gluconodelta lactone, or strong food grade hydrochloric acid. Alternately, thepH may be manipulated by adding bases such as sodium carbonate, sodiumbicarbonate or sodium hydroxide, or mixtures of these, for example.

Desirably, the surface of the uncoated particles attracts the firstcoating material, for example via electrostatic attraction. The firstcoating material deposits onto at least a portion of a surface of theparticles, thereby forming a layer of the coating material. Preferably,the first coating material forms a layer substantially covering theentire surface of at least some of the particles, and desirably of themajority, or substantially all, of the particles. The thickness of thislayer may be uniform or non-uniform.

The plant material coated with the first coating material is thencontacted with a solution of a second coating material. Prior to addingthe second coating material to the mixture containing the once-coatedplant material, or before the once-coated plant material is added to thesecond coating material, the overall electrical charge of the firstcoating on the plant material can be altered by adjusting the pH of theliquid medium. Suitable substances for adjusting the pH are acids andbases, e.g., weak organic acids such as acetic acid, adipic acid,fumaric acid, malic acid, lactic acid, tartaric acid, gluconic acids,and glucono delta lactone, or strong food grade hydrochloric acid, orbases such as sodium carbonate, sodium bicarbonate, or sodium hydroxide,for example. In one aspect, a layer of the first coating material (e.g.,a protein or protein hydrolyzate) can be treated with an acid tofacilitate electrostatic attraction of the second coating material.

The two coating materials may be mixed simultaneously with the plantmaterial. For example, a polysaccharide composition may be mixed with aprotein and with uncoated particles in the form of a suspension orsolution. Because of the coacervation mechanism (e.g., respectiveelectrostatic attractions and repulsions), the first coating materialcan deposit onto at least a portion of the surface of the particles andthe second coating material can attach onto at least a portion of theoutside surface of the layer.

The twice-coated plant material may be additionally coated with one ormore of the substances (which may optionally added along with the firstand/or second coating, or applied subsequently), with or withoutadditional additives. The additional additives that may be employed toadjust the physiological characteristics of the final product. Forexample, sweeteners like xylitol or solid sweeteners and solid flavors(encapsulated) can be added. Other food ingredients such as starches,polyols, oils, lipids, waxes, fats, fatty acids, glycerides, and thelike may be added to achieve desirable characteristics in the finalproduct.

In any of the embodiments described herein, the thickness of the layerof the first coating material may be uniform or non-uniform. Therelative amounts of plant particles and first and second coatingmaterials, as well as the types of each, may be adjusted to provide moreor less plant material and to control the properties of the resultingfilm, for example flexibility, strength, organoleptic attributes, etc.

A polysaccharide optionally contains at least one pectin. A pectin canform a complex coacervate with a protein as a result of hydrophobicinteractions and/or electrostatic complexation, in the presence or inthe absence of a salt, which can help to crosslink the pectin, formingthe pectin coating into a gel.

Alternatively, or in addition, first coating material and/or the secondcoating material can gel as a result of hydrogen bonding, hydrophobicinteractions, electrostatic interactions, formation of salt bridges(e.g., monovalent, divalent, or trivalent cation-induced crosslinkingresulting from the addition of, e.g., potassium, calcium, magnesium,and/or iron salts of chloride, citrate, lactate, acetates, and/or othercounterions), van der Waals interactions under room temperature orbelow, or during hot processing conditions, or some combination ofthese.

Gelation may be induced by various methods, such as adjusting the pH ofthe liquid medium containing the particles; adding monovalent, divalentor trivalent cations to the liquid medium containing the particles(which may be uncoated, coated with protein, or coated with protein andpolysaccharide at the time of addition); heating the particles to atemperature of between about 60° C. and about 90° C. for about 1 toabout 3 hours; cooling the particles to a temperature of between about20° C. and about 0° C. for about 1 to about 48 hours; removing at leastpart of the liquid medium from the coated particles by drying, e.g., byair drying, freeze drying, using reduced atmospheric pressure, orcombinations of these procedures.

In a particular embodiment, a salt may be added or included at least inpart to further assist in formation and gelation of a coacervate fromthe first and second coating materials. Examples of suitable salts mayinclude, but are not limited to, monovalent, divalent, or trivalentcations such as potassium, calcium, magnesium and iron, in the form ofsalts such as chloride, citrate, lactate or acetate salts. These saltsmay be used individually or in combination. In a particular embodiment,a divalent salt, such as salts of calcium and magnesium, can beintroduced during or after the addition of a polysaccharide compositionto the particles. The resulting coated particle may have a net negativeor neutral charge.

However, it has been found that the addition of such a salt is notnecessary in order for gel formation to occur when a polysaccharide suchas pectin is added to a protein layer. More specifically, gel formationis facilitated by specific interactions, believed to be betweencarboxylic groups of a polysaccharide and amino groups of proteins (orbetween amino groups of the polysaccharide and carboxylic groups of theproteins). This is particularly true under processing conditions of60-90° C. for 1-3 hours. The result of these interactions is that apolysaccharide-protein coacervate (and in particular, a pectin-proteincoacervate) may gel without the addition of divalent metal cations,which have been expected to be necessary for pectin gelation. Theseinteractions allow the gel strength of a pectin-protein coacervate to bemodified and controlled by, e.g., varying the number of availablecarboxylic groups and/or amine groups of the pectin, depending upon thenumber of carboxyl groups or amine groups in the protein able tointeract with them. This can be done by amidation or deamidation ofcarboxyl groups of the pectin, which can convert carboxyl groups tocarboxamides, or the converse, respectively.

In a preferred embodiment, at least one polysaccharide can form a gel inthe pH range between about 3 and about 9. Alternatively, or in addition,at least one polysaccharide can form a gel upon addition of monovalent,divalent or trivalent cations to the liquid medium during or afteraddition of the polysaccharide. Cations can be selected from the groupconsisting of potassium, calcium, magnesium and iron, and can beintroduced as chloride, citrate, lactate, and acetate salts that areadded to the liquid medium during or after addition of thepolysaccharide coating material to induce formation of the gel, e.g.,via formation of salt bridges. As described herein, gelation may also beinduced or aided by heating (e.g., to a temperature between about 60° C.and about 90° C., and preferably, between about 60° C. and about 80° C.,for about 10 to about 180 minutes, and preferably, for about 60 to about90 minutes). In particular, the use of commercially available pectins,at least in part, can reduce or eliminate the need for the addition of asalt, since such commercial pectins tend to gel immediately uponheating.

In a further embodiment, inducing gelation requires no active stepsbeyond mixing the desired components and allowing them to react for aperiod of time.

The process of forming the coacervate coating, or steps thereof, may berepeated, if desired, by using the same or different coating materialsas those described for the protein and polysaccharide coating materials,with or without the above-mentioned additional components or additives.A series of layers can therefore be built up around the base particle ofplant material, each of which may be the same or different from otherlayers, and which may provide desirable properties to the user, such asvarying flavor or chemesthetic effect, or further extension of flavorduration, as the successive layers of the coating come into contact withsaliva.

By using the methods disclosed herein, the strength of the coating ofthe particles of plant materials described herein, and thus, the coatingefficiency, can be controlled to achieve the desired release kineticsfor the plant material. In a particular embodiment, at least onepolysaccharide in the second coating can form a gel in the pH range ofabout 3 to about 9. In this embodiment, additional gel formation in thesecond coating layer may further improve the coating strength. Forinstance, κ-carrageenan can form a relatively strong and rigid gel undersimilar pH conditions, and may be included in a polysaccharide coatingmaterial. The amount of κ-carrageenan, which is preferably incorporatedin the coated particles in the range of about 10% to about 60% byweight, based on the total weight of the polysaccharides in the coatedparticles.

The strength of the gel matrix surrounding the particles may bemanipulated by modifying the above-described coating process. Inparticular, the second coating material may be preferentially optimizedin terms of the swelling behavior and visco-elasticity underphysiological pH and temperature conditions, for controlling theextraction kinetics of materials from the film.

In one embodiment of a method for making the film of coated particles ofplant material described herein, a protein is added to particles ofplant material in a liquid medium, forming a layer thereon. This layercan form on at least on a portion of a surface of the particles, andpreferably substantially cover the entirely surface of the particles.Thereafter, a pectin can be added to the protein-coated particlesobtained in the first step. The added pectin can be adsorbed onto atleast a portion of, and preferably all of, the surface of the firstlayer. At this stage, the pectin in the second coating may interact withthe protein in the first coating layer, thereby forming a coacervate.

As an extension of the above embodiment, κ-carrageenan can be added tothe liquid medium and adsorb onto at least a portion of a surface of thepectin, which in this instance forms a second coating layer. Preferably,the κ-carrageenan substantially covers the entire surfaces of the secondcoating layer. Then, κ-carrageenan may form a gel under appropriatecondition, resulting in a gel matrix comprising the plant material witha first coating of protein and a second coating of pectin, embedded inthe κ-carrageenan.

After formation, a gel matrix as described herein may desirably bestabilized by cooling or maintaining it at a temperature below thetemperature of gel formation, and preferably below room temperature, butabove the freezing point of the gel, and typically between about 20° C.and about 0° C., and preferably, between about 15° C. and about 5° C.,for about 1 to about 60 hours, and preferably, about 12 to about 48hours. Such stabilization may be performed before or after forming thefilm, or concurrently therewith.

Forming the Film

Following gelation, at least two different methods may be used to formthe film of encapsulated botanicals. In one embodiment, a complexcoacervate is formed into a relatively solid gel matrix, which is thencut along one or more sides into a desired geometry, followed by drying(e.g., at room temperature or freeze drying). Alternately, a complexcoacervate matrix can be squeezed and flattened (e.g., by passing itthrough rollers or by using a press) to provide a desired thickness, andoptionally cut to desired lengths and/or widths, with drying occurringbefore and/or after this flattening. In each case, it may be beneficialto have an excess of the second polymeric coating, which forms a gelmatrix around the first layer preferably substantially surrounding eachparticle of plant material. Additionally, an extrusion step may be usedin the film-formation process.

The film may be formed so to have a textured surface, and/orperforations. The film may also be cut after it is formed, either beforeor after optional drying.

If rollers are used to form the film, the rollers are optionally heatedrollers. The rollers may be smooth, or may be textured in order toprovide the above-mentioned texture and/or perforations to the film.

In a particular embodiment, the film of coated particles can desirablybe dried to a moisture content of less than about 15%, preferably, about2% to about 10%, and more preferably, about 2% to about 6%. Preferably,the drying is at room temperature or is freeze drying. Optionally, thedrying is conducted under less than one atmosphere of pressure.

The film may have nearly any desired dimensions. Preferably, the filmhas a size and strength so as to be self-supporting, meaning that it canwithstand normal handling while remaining intact. Also preferably, thefilm should be somewhat flexible. In an embodiment, the film received afurther coating after it is prepared.

The resulting films provide controlled release of the ingredients, and,by using different source materials prior to film formation, can includepatchworks of differing composition for different release profiles,ingredients, and the like, in a single film.

The film may be used itself as an orally enjoyable product, or may beincorporated into another product, such as a palatable or comestibleproduct. For example, the film may be used on the inside or outside ofan orally-enjoyed product, such as a pouched tobacco product.

Representative Compositions

In certain embodiments, the final composition of the film may containabout 10% to about 90% of plant material, more particularly about 20% toabout 80%, and still more particularly, about 40% to about 70% plantmaterial. The first layer may comprise an amount of the coated particleranging from about 1% to about 20%, more particularly about 1% to about30%, even more particularly about 5% to about 15%. The second coatingmay comprise an amount of the coated particle ranging from about 1% toabout 60%, more particularly about 5% to about 50%, even moreparticularly about 15% to about 40%. Each of these percentages isprovided as a percentage by weight based upon the dry weight of thefilm.

It may also be advantageous to add some additional components or otheradditives during the processing to affect the “mouth feel,” taste,texture, appearance, smell, flavor, flavor delivery and/or otherattributes of the plant material. One or more other components may beincluded in the coatings, including, but not limited to, the following:gum Arabic, flavorants, colorants, sweeteners such as xylitol, bulkingagents, fillers, anti-adherent compounds, dispersing agents, moistureabsorbing compounds, warming agents, cooling agents and film-formingagents. Other food ingredients such as starches, polyols, oils, lipids,waxes, fats, fatty acids, glycerides etc., may be also added to thecoating to enhance the mouth feel of the finished, dried product.Additives, such as physiological cooling agents, throat-soothing agents,spices, warming agents, tooth-whitening agents, breath-fresheningagents, vitamins, minerals, caffeine, drugs, and other actives may beincluded in any or all portions of the coatings. Such components may beused in amounts sufficient to achieve their intended effects.

The second coating material may be preferentially optimized forcontrolling the extraction kinetics of materials from the plant materialby controlling its swelling behavior and visco-elasticity underphysiological pH and temperature conditions. The release of selectedcompounds from the plant materials may be triggered by simple diffusioninto saliva, by action of enzymes in the saliva on one or more materialsmaking up the film, and/or upon application of pressure by the tongueand teeth. For example, upon ordinary chewing or dipping of the product,the user will release flavorings or other attributes as hydrationoccurs.

The coacervate coatings may be stable for a limited time, e.g., fromabout 10 to about 20 minutes under normal exposure to saliva. Thein-mouth time constant may be changed by selection of particularmaterials in the coatings.

Exemplary Method for Making Coated Particles.

FIG. 1 is a schematic depiction of a coated particle formed by themethod described herein. In the center is a finely-divided particle ofplant material, in this case tobacco, which has an overall negativecharge. It is surrounded or encapsulated by a first protein coatingmaterial, in this case, calcium caseinate. The protein layer is in turnsurrounded or encapsulated by a polysaccharide, in this caseκ-carrageenan. Potassium ions have been added to assist in formation ofthe gel.

FIG. 2 is a schematic depiction of one embodiment of the method offorming the coated particle. A micronized plant material 201 is combinedwith a first coating material 203 in a liquid medium to form a firstmixture 205 of coated plant material. If needed, the first mixture 205is treated to adjust the pH in 207 prior to the contact with the secondcoating material 209 to form a second mixture in 211. If desired,additional material 213 may be added to the second mixture to impartadditional characteristics to the finished coated plant material, or toaid in gelation of the outer coating(s). The pH of the resultingmaterial may be adjusted in 215 by addition of a suitable food-gradeacid, base, or salt. Water may be added in 219, or removed prior to,after, or concurrently with forming the gel 217, followed by forming afilm 221 from the gel of coated particles. The film may be optionallydried 223 and then utilized as is, or can be incorporated into otherproducts.

For example, a solution containing about 0.5 to about 2% (w/w) proteinin deionized water is prepared. The divided plant material is dispersedin the protein solution. The pH is adjusted to within the range fromabout 3.5 to about 6 with citric acid, depending on the protein used.The selected second coating material is added to the mix in a powder orsolution form and mixed thoroughly. The resulting mixture is heated atabout 70° C. to about 80° C. for about 1 to about 2 hours, depending onthe protein used. A salt may be added to the heated mix for propergelation of the carbohydrate. Salts are preferably added to coacervatesbased on carrageenan, while pectin-based coacervate gels may or may notneed any added salt. Suitable salts can include KCl, calcium lactate, ora mixture of KCl and calcium lactate, depending on the type ofcarbohydrate used. Other salts of bivalent metals such as calciumchloride or calcium citrate (including magnesium salts) can be used aswell. The coacervate gel is preferably refrigerated for about 12 toabout 48 hours before being processed into a film.

In another embodiment, there is provided a method of preparing anorally-enjoyable film of coated particles of plant material whichcomprises dissolving a first coating material in a liquid medium and ifnecessary, adjusting the pH of the resulting mixture to within a firstpredetermined range; dispersing a colloidal plant material in themedium, either as a dry particle or in the form of a colloidaldispersion, and if necessary adjusting the pH of the resulting mixtureto within a second predetermined range; dispersing a second coatingmaterial in the medium and if necessary adjusting the pH of theresulting mixture to within a third predetermined range; optionallyheating the resulting mixture at a temperature of up to the boilingpoint of water, preferably about 60° C. to about 90° C., for about 10minutes to about 180 minutes or more; refrigerating the mixture at atemperature of down to about the freezing point of the liquid mixture,preferably about 20° C. to about 0° C., and more preferably from about15° C. to about 2° C. for about 1 to about 48 hours, then optionallyremoving excess liquid before forming a film. Additional liquid mayoptionally be removed following film formation.

An orally-enjoyable film as described herein is preferably stable in themouth for about 1 to about 20 minutes. The extraction mechanics of theplant material in the mouth may be altered by altering one or more ofthe following characteristics of the coatings: swelling behavior,visco-elasticity under physiological pH and temperature conditions,porosity, stability or rate of diffusion of ingredients underapplication of pressure by tongue or teeth or both, stability fromdissolution upon attack from enzymes in saliva, or combinations ofthese. Also, one or more of the following characteristics of thecoatings can be optimized for controlling the mouth feel of the edibleproduct: slipperiness, sliminess, firmness, sponginess, stability orrate of diffusion of ingredients under application of pressure by tongueor teeth or both, stability from dissolution upon attack from enzymes insaliva, or combinations of these. These properties can be varied byselecting various first and second coating materials, combiningdifferent coating materials, modifying the properties of coatingmaterials, e.g., by crosslinking, or combinations of these.

EXAMPLES Example 1

This Example provides a general method used in the subsequent Examples,wherein lowercase letters in parentheses denote the various ingredients.First, a protein (a) solution in deionized water has in it suitablydivided plant material (b), and the pH of the mixture is adjusted towithin the range of 3.5 to 6 by adding citric acid (c). The secondcoating material, such as a carbohydrate in powder or solution form (d),is added and the resulting mixture is heated at about 70° C. to about80° C. for about 1 hour to about 2 hours to form a coacervate gelcontaining protein-coated plant particles. Depending on the proteinused, one or more salts (e, f) such as potassium chloride and/or saltsof bivalent metals such as calcium chloride, calcium citrate, calciumlactate, or magnesium salts may optionally be used. When one of thecoatings is a carrageenan or alginate, it may be preferable to add asalt to allow gelation of the mixture, whereas if the gel is pectinbased, addition of a salt may not be needed. Coacervate gels may or maynot need any added salt. The coacervate gel is refrigerated for about 12hours to about 48 hours to condition it before forming the film.

Example 2

Ground tea powder encapsulation: Basis 100 gm of coacervate gel.Na-caseinate—κ-carrageenan coacervate gel encapsulating tea powder.Deionized water=89.34 gm.(a) Na-caseinate, low fat (from American Casein company)=0.89 gm.(b) Ball milled tea powder, average particle size 1 micron=4.47 gm.(c) 0.5 M Citric acid solution (Sigma, 99% pure)=0-2.68 gm.(d) κ-carrageenan (FMC Biopolymers Gelcarin 911 NF)=2.23 gm.(e) 0.5 M KCl (ACS grade, Fisher) solution=0.18 gm.(f) 0.153 M Calcium lactate solution (Sigma, 90%)=0.20 gm.

Example 3

Ground coffee powder encapsulation: Basis 100 gm of coacervate gel.Na-caseinate—κ-carrageenan coacervate gel encapsulating coffee powderDeionized water=89.34 gm.(a) Na-caseinate, low fat (from American Casein company)=0.89 gm.(b) Ball milled coffee powder, 1 micron=4.47 gm.(c) 0.5 M Citric acid solution (Sigma, 99% pure)=2.68 gm.(d) κ-carrageenan (FMC Biopolymers Gelcarin 911 NF)=2.23 gm.(e) 0.5 M KCl (ACS grade, Fisher) solution=0.18 gm.(f) 0.153 M Calcium lactate solution (Sigma, 90%)=0.20 gm.

Example 4

Tobacco powder encapsulation: Basis 100 gm of coacervate gel.Na-caseinate—κ-carrageenan coacervate gel encapsulating tobacco powderDeionized water=83.42 gm.(a) Na-caseinate, low fat (from American Casein company)=0.83 gm.(b) 400 mesh ground burley tobacco=5.84 gm.(c) 0.5 M Citric acid solution (Sigma, 99% pure)=7.95 gm.(d) κ-carrageenan (FMC Biopolymers Gelcarin 911 NF)=1.67 gm.(e) 0.5 M KCl (ACS grade, Fisher) solution=0.14 gm.(f) 0.153 M Calcium lactate solution (Sigma, 90%)=0.15 gm.

Example 5

Tobacco powder encapsulation: Basis 100 gm of coacervate gel.Na-caseinate—κ-carrageenan coacervate gel encapsulating tobacco powderDeionized water=86.77 gm.(a) Na-caseinate, low fat (from American Casein company)=0.87 gm.(b) 400 mesh ground burley tobacco=5.21 gm.(c) 0.5 M citric acid solution (Sigma, 99% pure)=4.07 gm.(d) κ-carrageenan (FMC Biopolymers Gelcarin 379 NF)=2.6 gm.(e) 0.153 M Calcium lactate solution (Sigma, 90%)=0.49 gm.

Example 6

Tobacco powder encapsulation: Basis 100 gm of coacervate gel.Gelatin—pectin coacervate gel encapsulating tobacco powderDeionized water=86.96 gm.(a) Gelatin from porcine skin, type A, 300 Bloom=0.87 gm.(b) 400 mesh ground burley tobacco=6.09 gm.(c) 0.5 M citric acid solution (Sigma, 99% pure)=1.47 gm.(d) Citrus peel Pectin, 40% ester (CP Kelco Genu pectin LM-18-CG)=1.74gm.(e) 0.153 M calcium lactate solution (Sigma, 90%)=2.87 gm.

Example 7

Tobacco powder encapsulation: Basis 100 gm of coacervate gel.Na-caseinate—pectin coacervate gel encapsulating tobacco powderDeionized water=84.78 gm.(a) Na-caseinate, low fat (from American Casein company)=0.85 gm.(b) 400 mesh ground burley tobacco=5.93 gm.(c) 0.5 M citric acid solution (Sigma, 99% pure)=6.74 gm.(d) Apple Pectin, 6% ester (Sigma)=1.70 gm

Example 8

Tobacco powder encapsulation: Basis 100 gm of coacervate gel.Na-caseinate—pectin coacervate gel encapsulating tobacco powderDeionized water=84.81 gm.(a) Na-caseinate, low fat (from American Casein company)=0.85 gm.(b) 400 mesh ground burley tobacco=5.94 gm.(c) 0.5 M citric acid solution (Sigma, 99% pure)=6.71 gm.(d) Amidated low ester pectin (Genu pectin X-916-02)=1.70 gm.

Example 9

Tobacco powder encapsulation: Basis 100 gm of coacervate gel.Chitosan—pectin coacervate gel encapsulating tobacco powderDeionized water=82.03 gm.(a) Chitosan, medium viscosity (Vanson)=0.82 gm.(b) 400 mesh ground burley tobacco=5.74 gm.(c) 0.5 M citric acid solution (Sigma, 99% pure)=9.61 gm.(d) Apple Pectin, 6% ester (Sigma)=1.80 gm.

Example 10

Tobacco powder encapsulation: Basis 100 gm of coacervate gel.Soy isolate—κ-carrageenan coacervate gel encapsulating tobacco powderDeionized water=83.25 gm.(a) Soy isolate (Solae company, Supro EX-38)=0.83 gm.(b) 400 mesh ground burley tobacco=5.83 gm.(c) 0.5 M citric acid solution (Sigma, 99% pure)=8.14 gm.(d) κ-carrageenan (FMC Biopolymers Gelcarin 911 NF)=1.66 gm.(e) 0.5 M KCl (ACS grade, Fisher) solution=0.14 gm.(f) 0.153 M Calcium lactate solution (Sigma, 90%)=0.15 gm.

Example 11

Tobacco powder encapsulation: Basis 100 gm of coacervate gelSoy concentrate—κ-carrageenan coacervate gel encapsulating tobaccopowder.Deionized water=83.56 gm.(a) Soy concentrate (Solae company, Alpha 10)=0.84 gm.(b) 400 mesh ground burley tobacco=5.85 gm.(c) 0.5 M citric acid solution (Sigma, 99% pure)=7.80 gm.(d) κ-carrageenan (FMC Biopolymers Gelcarin 911 NF)=1.67 gm.(e) 0.5 M KCl (ACS grade, Fisher) solution=0.14 gm.(f) 0.153 M calcium lactate solution (Sigma, 90%)=0.15 gm.

Example 12

Tobacco powder encapsulation: Basis 100 gm of coacervate gelSoy isolate—pectin coacervate gel encapsulating tobacco powderDeionized water=84 gm.(a) Soy isolate (Solae company, Supro EX 38)=0.83-1.8 gm.(b) 400 mesh ground burley tobacco=5.78 gm.(c) 0.5 M citric acid solution (Sigma, 99% pure)=6.58 gm.(d) Tobacco sourced pectin=1.87 gm.(e) 0.153 M Calcium lactate solution (Sigma, 90%)=0-2.77 gm.

Example 13

Tobacco powder encapsulation: Basis 100 gm of coacervate gel.Tobacco sourced protein—κ-carrageenan coacervate gel encapsulatingtobacco powderDeionized water=87.05 gm.(a) Tobacco sourced protein, (Philip Morris Company)=0.87 gm.(b) 400 mesh ground burley tobacco=6.16 gm.(c) 0.5 M citric acid solution (Sigma, 99% pure)=3.87 gm.(d) κ-carrageenan (FMC Biopolymers Gelcarin 911 NF)=1.76 gm.(e) 0.5 M KCl (ACS grade, Fisher) solution=0.15 gm.(f) 0.153 M Calcium lactate solution (Sigma, 90%)=0.15 gm.

Example 14

Tobacco powder encapsulation: Basis 100 gm of coacervate gel.Tobacco sourced protein—pectin coacervate gel encapsulating tobaccopowderDeionized water=86.13 gm.(a) Tobacco sourced protein, (Philip Morris Company)=0.86 gm.(b) 400 mesh ground burley tobacco=6.10 gm.(c) 0.5 M Citric acid solution (Sigma, 99% pure)=5.17 gm.(d) 40% ester pectin (Genu pectin LM-18-CG-Z)=1.74 gm.

Example 15

Tobacco powder encapsulation: Basis 100 gm of coacervate gel.Na-caseinate—κ-carrageenan coacervate gel encapsulating ball milled DBCbright tobacco powderDeionized water=83.42 gm.(a) Na-caseinate, low fat (from American Casein company)=0.83 gm.(b) Ball milled DBC Bright tobacco, 1 micron=5.84 gm.(c) 0.5 M Citric acid solution (Sigma, 99% pure)=7.95 gm.(d) κ-carrageenan (FMC Biopolymers Gelcarin 911 NF)=1.67 gm.(e) 0.5 M KCl (ACS grade, Fisher) solution=0.14 gm.(f) 0.153 M Calcium lactate solution (Sigma, 90%)=0.15 gm.

Example 16

Tobacco powder encapsulation: Basis 100 gm of coacervate gel.Na-caseinate—κ-carrageenan coacervate gel encapsulating tobacco powderprocessed via Microfluidics HomogenizerDeionized water=83.42 gm.(a) Na-caseinate, low fat (from American Casein company)=0.83 gm.(b) 400 mesh ground burley tobacco, processed via Microfluidics, ˜15micron=5.84 gm.(c) 0.5 M Citric acid solution (Sigma, 99% pure)=7.95 gm.(d) κ-carrageenan (FMC Biopolymers Gelcarin 911 NF)=1.67 gm.(e) 0.5 M KCl (ACS grade, Fisher) solution=0.14 gm.(f) 0.153 M Calcium lactate solution (Sigma, 90%)=0.15 gm.

Information regarding the extraction, deesterfication, and amidation oftobacco pectins may be found in U.S. Pat. Nos. 4,034,764; 4,143,666;4,972,854; 4,506,684; and/or 5,724,998, each of which is incorporatedherein by reference.

While various methods and products have been described herein withreference to specific embodiments, variations and modifications may bemade without departing from the spirit and the scope of the appendedclaims. Such variations and modifications are to be considered withinthe purview and scope of the invention as defined by the appendedclaims.

1. A method for preparing an orally-enjoyable film of coated particlesof finely divided plant material, comprising: combining particles offinely divided plant material and a first coating material in a liquidmedium, wherein the first coating material adsorbs onto at least aportion of a surface of the particles to form a layer of the firstcoating material; mixing a second coating material with the liquidmedium, wherein the second coating material adsorbs onto at least aportion of the layer; inducing gelation to form a gel matrix comprisingthe particles at least partially surrounded by the layer of the firstcoating material and embedded in the second coating material; andforming a film from the gel matrix, wherein: (i) the plant material andthe first coating material are electrostatically attracted, (ii) thefirst coating material and the second coating material areelectrostatically attracted, or (iii) both (i) and (ii).
 2. The processof claim 1, wherein said forming the film comprises: (i) cutting saidgel matrix into a desired geometry, and/or (ii) flattening said gelmatrix.
 3. The process of claim 1 wherein said forming comprisesflattening using one or more rollers, and at least one of the rollers isheated and/or is textured.
 4. The process of claim 1, wherein said plantmaterial consists of: (i) an extract from a plant; or (ii) a micronizedpowder obtained by finely dividing a plant or a fragment of a plant. 5.The process of claim 1, wherein said plant material and said firstcoating material are electrostatically attracted and said first coatingmaterial and said second coating material are electrostaticallyattracted.
 6. The process of claim 1, wherein: (i) said first coatingmaterial comprises at least one protein selected from the groupconsisting of milk protein, whey protein, soy protein, wheat protein,rice protein, egg white protein, protein obtained from tobacco, gelatin,and protein hydrolyzates; (ii) said first coating material comprises azwitterionic or positively charged protein; (iii) said second coatingcomprises at least one pectin obtained from tobacco, apples, citruspeel, plums, or gooseberries; (iv) said second coating comprises ananionic polysaccharide; (v) said second coating comprises at least onematerial selected from the group consisting of carrageenans, gum Arabic,carboxymethyl cellulose, sodium alginates, gum tragacanth, locust beangum, gellan gum, and xanthan gum; (vi) said plant material comprises atobacco, a tobacco substitute, coffee, or tea; (vii) said film isself-supporting; (viii) further comprising adding a flavorant; (ix) saidfilm comprises a smooth surface and/or a textured surface and/orperforations; (x) said film is formed from two or more gel matrices ofdifferent compositions; (xi) two or more of (i) through (x).
 7. Theprocess of claim 1: (i) wherein said process is performed withoutaddition of a salt as a crosslinking agent; (ii) further comprisingforming a colloidal dispersion of said plant material; (iii) furthercomprising lowering the pH of said liquid medium using a materialselected from the group consisting of acetic acid, adipic acid, fumaricacid, malic acid, lactic acid, tartaric acid, gluconic acid, gluconodelta lactone, hydrochloric acid, and mixtures thereof; (iv) furthercomprising increasing the pH of said liquid medium using a materialselected from the group consisting of sodium carbonate, sodiumbicarbonate, sodium hydroxide, and mixtures of these; (v) furthercomprising a drying step; (vi) further comprising an extrusion step;(vii) further comprising using at least a third coating material to formone or more additional layers around the plant material; or (viii) twoor more of (i) through (vii).
 8. The process of claim 1, furthercomprising inducing gelation by (i) adjusting a pH of said liquidmedium; (ii) adding monovalent, divalent, or trivalent cations to saidliquid medium; (iii) heating to a temperature of between about 60° C.and about 90° C. for about 1 to about 3 hours; (iv) cooling to atemperature of between about 20° C. and about 0° C. for about 1 to about48 hours; or (v) two or more of (i) to (iv).
 9. The process of claim 1,wherein, (i) said first coating material is selected from the groupconsisting of proteins, cationic polysaccharides or oligosaccharides,non-ionic polysaccharides, oligosaccharides, and mixtures thereof; (ii)said second coating material is selected from the group consisting ofanionic, zwitterionic, or neutral polysaccharides; a protein; andmixtures thereof; or (iii) (i) and (ii).
 10. The process of claim 9,wherein said first coating material is a protein and said second coatingmaterial is a polysaccharide.
 11. An orally-enjoyable film of coatedparticles of finely-divided plant material, the film comprising: amatrix comprising particles of finely-divided plant material at leastpartially surrounded by a first coating material and embedded in asecond coating material, wherein: (i) the plant material and the firstcoating material are electrostatically attracted, (ii) the first coatingmaterial and the second coating material are electrostaticallyattracted, or (iii) both (i) and (ii).
 12. The film of claim 11, whereinsaid plant material consists of: (i) an extract from a plant; or (ii) amicronized powder obtained by finely dividing a plant or a fragment of aplant.
 13. The film of claim 11, wherein: (i) said particles have anaverage largest dimension of less than about 3000 microns; (ii) saidfilm comprises: (a) said plant material in an amount of about 10 toabout 90% by dry weight, (b) first coating material in an amount ofabout 1% to about 20% by dry weight, and/or (c) second coating materialin an amount of about 5% to about 50% by dry weight; (iii) the coatedbase particle has a moisture content of less than about 15% by weight;(iv) the coated particle has a net negative or neutral charge; (v)further comprising one or more additional layers around the plantmaterial; or (vi) two or more of (i) to (v).
 14. The film of claim 11,wherein: (i) said first coating material comprises at least one proteinselected from the group consisting of milk protein, whey protein, soyprotein, wheat protein, rice protein, egg white protein, proteinobtained from tobacco, gelatin, and protein hydrolyzates; (ii) saidfirst coating material comprises a zwitterionic or positively chargedprotein; (iii) said second coating comprises at least one pectinobtained from tobacco, apples, citrus peel, plums, or gooseberries; (iv)said second coating comprises an anionic polysaccharide; (v) said secondcoating comprises at least one material selected from the groupconsisting of carrageenans, gum Arabic, carboxymethyl cellulose, sodiumalginates, gum tragacanth, locust bean gum, gellan gum, and xanthan gum;(vi) said plant material comprises a tobacco, a tobacco substitute,coffee, or tea; (vii) said film is self-supporting; (viii) furthercomprising at least a third coating material forming at least a secondlayer around the plant material; (ix) further comprising a flavorant;(x) said film comprises a smooth surface and/or a textured surfaceand/or perforations; (xi) said film comprises two or more matrices ofdifferent compositions; or (xii) two or more of (i) through (xi). 15.The film of claim 11, wherein the plant material comprises tobacco, atobacco substitute, or a combination thereof.
 16. The film of claim 11,wherein, (i) said first coating material is selected from the groupconsisting of proteins, cationic polysaccharides or oligosaccharides,non-ionic polysaccharides, oligosaccharides, and mixtures thereof; (ii)said second coating material is selected from the group consisting ofanionic, zwitterionic, or neutral polysaccharides; a protein; andmixtures thereof; or (iii) (i) and (ii).
 17. The film of claim 16,wherein said first coating material is a protein and said second coatingmaterial is a polysaccharide.
 18. The film of claim 17, wherein saidprotein has a molecular weight of between about 2 kDa and about 1000 kDaand said polysaccharide has a molecular weight of between about 5 kDaand about 1000 kDa.
 19. A palatable or comestible product comprising atleast one film according to claim 11.